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Comparative Investigations of Cp*-Based Group 9 Metal-Catalyzed Direct C–H Amination of Benzamides
Figg, Travis M.,Park, Sehoon,Park, Juhyeon,Chang, Sukbok,Musaev, Djamaladdin G. American Chemical Society 2014 Organometallics Vol.33 No.15
<P>Key mechanistic features of the [Cp*MCl<SUB>2</SUB>]<SUB>2</SUB> (M = Ir, Rh, Co; all are in group 9) catalyzed C–H amination of benzamides with organic azides were investigated with a strong emphasis on the <I>metal effects on the</I> <I>reaction</I> <I>mechanism</I>, revealing that the Rh- and Ir-catalyzed reactions follow a similar reaction profile, albeit with different individual kinetic and thermodynamic parameters. The observation that the Ir-based system was much superior in terms of the rates and efficiency in comparison to Rh was attributed to <I>the intrinsically strong relativistic effects in iridium.</I> While a cobalt system [Cp*Co<SUP>III</SUP>] showed <I>little</I> catalytic activity for most azides examined, plausible [(BA)(Cp*)CoNR]<SUP>+</SUP> intermediates of these reactions were characterized as a “Co(III)-nitrenoid radical” species with a weak (“one electron–two center type”) Co–NPh bond. Its Rh and Ir analogues are characterized as diamagnetic metal nitrenoids with a strong MNR double bond. The provided experimental and computational investigations indicate that the rate-limiting step of the reaction resides in the final stage (protodemetalation) that takes place via a concerted metalation–deprotonation (CMD) mechanism. While experimental measurements of thermodynamic parameters were in good agreement with DFT calculations, theoretical predictions on the electronic nature of key intermediates and energy barriers were successfully used to rationalize the experimentally observed reactivity pattern.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/orgnd7/2014/orgnd7.2014.33.issue-15/om5005868/production/images/medium/om-2014-005868_0012.gif'></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/om5005868'>ACS Electronic Supporting Info</A></P>
The method of interpolation and compression for DSP
Musaev M.M.,Rahmatov F.A. 대한전자공학회 2008 ICEIC:International Conference on Electronics, Inf Vol.1 No.1
There are problems of the frequency drift of sampling, compression or low-frequency filtration in working up of continuous signals on DSP. In many problems of investigation and analysis the form of signal presentation or its details in the form of analytical description is needed. The solution of the problems with traditional methods is quite difficult because of many operations and complications in modern DSP. Within the scope of linear theory the transmission of signal or its fragment into the spectral sphere with one of the discrete basis of Fourier-analysis is given. Further the signal spectrum of given algorithm transforms into the algebraic polynomial. This allows us solve the majority of shown problems of digital signal processing on DSP.